M−N 3 Configuration on Boron Nitride Boosts Singlet Oxygen Generation via Peroxymonosulfate Activation for Selective Oxidation

作者：Jianzheng Zhen, Jiahao Sun, Xiangwei Xu, Zenglong Wu, Wenkai Song, Yunzhan Ying, Shikun Liang, Lingshan Miao, Jiazhen Cao, Weiyang Lv, Weiyang Lv, Changsheng Song, Changsheng Song, Yuyuan Yao, Mingyang Xing · 发表于：Angewandte Chemie International Edition · 年份：2024 · DOI：10.1002/anie.202402669 · 被引用次数：185 · 研究领域：Catalytic Processes in Materials Science、Electrocatalysts for Energy Conversion、Advanced oxidation water treatment

Abstract Singlet oxygen ( 1 O 2 ) is an essential reactive species responsible for selective oxidation of organic matter, especially in Fenton‐like processes. However, due to the great limitations in synthesizing catalysts with well‐defined active sites, the controllable production and practical application of 1 O 2 remain challenging. Herein, guided by theoretical simulations, a series of boron nitride‐based single‐atom catalysts (BvBN/M, M=Co, Fe, Cu, Ni and Mn) were synthesized to regulate 1 O 2 generation by activating peroxymonosulfate (PMS). All the fabricated BvBN/M catalysts with explicit M−N 3 sites promoted the self‐decomposition of the two PMS molecules to generate 1 O 2 with high selectivity, where BvBN/Co possessed moderate adsorption energy and d ‐band center exhibited superior catalytic activity. As an outcome, the BvBN/Co‐PMS system coupled with membrane filtration technology could continuously transform aromatic alcohols to aldehydes with nearly 100 % selectivity and conversion rate under mild conditions, suggesting the potential of this novel catalytic system for green organic synthesis.